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采用沉淀法和浸渍法制备了2种铬基(Cr2O3和CrO3/Cr2O3)催化剂,用于气相氟化2-氯-1,1,1-三氟乙烷合成1,1,1,2-四氟乙烷。研究发现含有低价铬(Cr3+)物种的Cr2O3催化剂上2-氯-1,1,1-三氟乙烷的稳态转化率为18.5%,而含有高价铬(Cr6+)物种和低价铬(Cr3+)物种的CrO3/Cr2O3催化剂初始转化率达到30.6%,然而存在明显的失活。含有Cr6+物种的CrO3/Cr2O3催化剂的2-氯-1,1,1-三氟乙烷氟化反应初始TOF值为1.71×10-4 molHCFC-133a·molCr(Ⅵ)-1·s-1,高于含有Cr3+物种的Cr2O3催化剂(4.16×10-5 molHCFC-133a·molCr(Ⅲ)-1·s-1)。Cr2O3催化剂在氟化反应前后催化剂的物相结构保持不变;而含有高价铬物种的CrO3/Cr2O3催化剂经HF反应后生成了CrOxFy活性物种。然而,CrOxFy物种在反应中挥发或转化成稳定但无活性的CrF3,从而导致催化剂失活。 相似文献
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采用密度泛函理论计算方法模拟了简单钴卟啉过氧中间体PCo-O2与环己烷C6H12的作用,分析了反应路径中各驻点能量和反应过渡态分子构型。研究结果表明,PCo-O2向底物环己烷夺氢的反应可以延正方向进行,二线态PCo-O2更具反应活性,反应过程中Co-O键得到加强,O-O键被削弱。依据理论计算结果,探讨了四苯基钴卟啉催化环己烷氧化生成环己醇和环己酮的反应机理,指出反应延Lyons高价金属氧代物机理生成环己醇,而反应循环中产生的烷基自由基可以延烷基过氧化过渡金属配合物反应机理进行生成环己酮。 相似文献
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Effect of substrate temperature on microstructure and optical properties of single-phased Ag20 film deposited by using radio-frequency reactive magnetron sputtering method 下载免费PDF全文
Using a radio-frequency reactive magnetron sputtering technique, a series of the single-phased Ag20 films are deposited in a mixture of oxygen and argon gas with a flow ratio of 2:3 by changing substrate temperature (Ts). Effects of the Ts on the microstructure and optical properties of the films are investigated by using X-ray diffractometry, scanning electron microscopy and spectrophotometry. The single-phased Ag20 films deposited at values of Ts below 200℃ are (111) preferentially oriented, which may be due to the smallest free energy of the (111) crystalline face. The film crystallization becomes poor as the value of Ts increases from 100℃ to 225℃. In particular, the Ag20 film deposited at Ts=225℃ loses the (111) preferential orientation. Correspondingly, the film surface morphology obviously evolves from a uniform and compact surface structure to a loose and gullied surface structure. With the increase of Ts value, the transmissivity and the reflectivity of the films in the transparent region are gradually reduced, while the absorptivity gradually increases, which may be attributed to an evolution of the crystalline structure and the surface morphology of the films. 相似文献
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